Highly efficient and selective absorption of H2S in phenolic ionic liquids: A cooperative result of anionic strong basicity and cationic hydrogenbond donation

被引:121
作者
Huang, Kuan [1 ,2 ]
Zhang, Xiao-Min [3 ]
Zhou, Lin-Sen [4 ]
Tao, Duan-Jian [5 ]
Fan, Jie-Ping [1 ,2 ]
机构
[1] Nanchang Univ, Minist Educ, Poyang Lake Key Lab Environm & Resource Utilizat, Nanchang 330031, Jiangxi, Peoples R China
[2] Nanchang Univ, Sch Resources Environm & Chem Engn, Nanchang 330031, Jiangxi, Peoples R China
[3] Nanjing Univ, Sch Chem & Chem Engn, Nanjing 210093, Jiangsu, Peoples R China
[4] China Acad Engn Phys, Inst Mat, Ctr Interface Dynam Sustainabil, Chengdu 610200, Sichuan, Peoples R China
[5] Jiangxi Normal Univ, Coll Chem & Chem Engn, Nanchang 330022, Jiangxi, Peoples R China
关键词
Selective absorption; Hydrogen sulfide; Carbon dioxide; Phenolic ionic liquids; Hydrogen-bond donation; CARBON-DIOXIDE; AQUEOUS-SOLUTIONS; SULFIDE SOLUBILITY; CO2; METHYLDIETHANOLAMINE; MONOETHANOLAMINE; SEPARATION; CAPTURE; MIXTURE; HEXAFLUOROPHOSPHATE;
D O I
10.1016/j.ces.2017.07.048
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
A series of phenolic ILs containing different cations were synthesized and investigated for the absorption of H2S and CO2 in this work. It is interestingly found that the solubilities of H2S in these phenolic ILs are comparably high because of the strong interaction of basic phenolate anion with acidic H2S, while the solubilities of CO2 decrease significantly with the increase of cationic hydrogen-bond donation. Tetramethylguanidinium phenolate ([TMGH][PhO]), which is constructed with anion of strong basicity and cation of strong hydrogen-bond donating ability, is thus highlighted with both high solubilities of H2S (0.56 mol/mol at 313.2 K and 0.1 bar, and 0.85 mol/mol at 313.2 K and 1 bar) and high selectivities of H2S/CO2 (6.2 for the ratio of H2S solubility at 313.2 K and 0.1 bar vs. CO2 solubility at 313.2 K and 1 bar, and 9.4 for the ratio of H2S solubility at 313.2 K and 1 bar vs. CO2 solubility at 313.2 K and 1 bar). Owing to the small molecular size of [TMGH][PhO], the absolute solubilities of H2S in it (2.68 mol/kg at 313.2 K and 0.1 bar, and 4.08 mol/kg at 313.2 K and 1 bar) are particularly fascinating, and much higher than other absorbents reported in the literature. Furthermore, [TMGH][PhO] is costeffective in comparison with other functionalized ILs specifically designed for H2S capture, since it can be facilely synthesized from the one-step neutralization of readily available 1,1,3,3tetramethylguanidine and phenol. The results obtained in this work indicate that [TMGH][PhO] is a promising candidate for the selective sweetening of natural gas. (C) 2017 Elsevier Ltd. All rights reserved.
引用
收藏
页码:253 / 263
页数:11
相关论文
共 56 条
[1]   Simultaneous measurement absorption of CO2 and H2S mixture into aqueous solutions containing Diisopropanolamine blended with 1-butyl-3-methylimidazolium acetate ionic liquid [J].
Afsharpour, Alireza ;
Haghtalab, Ali .
INTERNATIONAL JOURNAL OF GREENHOUSE GAS CONTROL, 2017, 58 :71-80
[2]   Estimation of H2S solubility in ionic liquids using a rigorous method [J].
Ahmadi, Mohammad Ali ;
Haghbakhsh, Reza ;
Soleimani, Reza ;
Bajestani, Majid Bazrgar .
JOURNAL OF SUPERCRITICAL FLUIDS, 2014, 92 :60-69
[3]   Connectionist technique estimates H2S solubility in ionic liquids through a low parameter approach [J].
Ahmadi, Mohammad-Ali ;
Pouladi, Behzad ;
Javvi, Yahya ;
Alfkhani, Shahab ;
Soleimani, Reza .
JOURNAL OF SUPERCRITICAL FLUIDS, 2015, 97 :81-87
[4]  
Bara J. E., 2012, POTENTIAL HYDROGEN S, VII, P155, DOI DOI 10.1007/978-94-007-2891-2
[5]   Ionic liquids: Innovative fluids for chemical processing [J].
Brennecke, JF ;
Maginn, EJ .
AICHE JOURNAL, 2001, 47 (11) :2384-2389
[6]   Capture of H2S from Binary Gas Mixture by Imidazolium-Based Ionic Liquids with Nonfluorous Anions: A Theoretical Study [J].
Chen, Jie-Jie ;
Li, Wen-Wei ;
Yu, Han-Qing ;
Li, Xue-Liang .
AICHE JOURNAL, 2013, 59 (10) :3824-3833
[7]   Testing solubility data of H2S and SO2 in ionic liquids for sulfur-removal processes [J].
Faundez, Claudio A. ;
Diaz-Valdes, Joaquin F. ;
Valderrama, Jose O. .
FLUID PHASE EQUILIBRIA, 2014, 375 :152-160
[8]   Thermophysical properties of imidazolium-based ionic liquids [J].
Fredlake, CP ;
Crosthwaite, JM ;
Hert, DG ;
Aki, SNVK ;
Brennecke, JF .
JOURNAL OF CHEMICAL AND ENGINEERING DATA, 2004, 49 (04) :954-964
[9]  
Frisch M.J., 2016, Gaussian, V16
[10]   Protic ionic liquids: Properties and applications [J].
Greaves, Tamar L. ;
Drummond, Calum J. .
CHEMICAL REVIEWS, 2008, 108 (01) :206-237